[1] We present a global tabulation of black carbon (BC) and primary organic carbon (OC) particles emitted from combustion. We include emissions from fossil fuels, biofuels, open biomass burning, and burning of urban waste. Previous ‘‘bottom-up’’ inventories of black and organic carbon have assigned emission factors on the basis of fuel type and economic sector alone. Because emission rates are highly dependent on combustion practice, we consider combinations of fuel, combustion type, and emission controls and their prevalence on a regional basis. Central estimates of global annual emissions are 8.0 Tg for black carbon and 33.9 Tg for organic carbon. These estimates are lower than previously published estimates by 25–35%. The present inventory is based on 1996 fuel-use data, updating previous estimates that have relied on consumption data from 1984. An offset between decreased emission factors and increased energy use since the base year of the previous inventory prevents the difference between this work and previous inventories from being greater. The contributions of fossil fuel, biofuel, and open burning are estimated as 38%, 20%, and 42%, respectively, for BC, and 7%, 19%, and 74%, respectively, for OC. We present a bottom-up estimate of uncertainties in source strength by combining uncertainties in particulate matter emission factors, emission characterization, and fuel use. The total uncertainties are about a factor of 2, with uncertainty ranges of 4.3–22 Tg/yr for BC and 17–77 Tg/yr for OC. Low-technology combustion contributes greatly to both the emissions and the uncertainties. Advances in emission characterization for small residential, industrial, and mobile sources and topdown analysis combining field measurements and transport modeling with iterative inventory development will be required to reduce the uncertainties further. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; KEYWORDS: emission, black carbon, organic carbon, fossil fuel, biofuel, biomass burning

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A technology-based global inventory of black and organic carbon emissions from combustion

The application of mass spectrometric techniques to the realtime measurement and characterization of aerosols represents a significant advance in the field of atmospheric science. This review focuses on the aerosol mass spectrometer (AMS), an instrument designed and developed at Aerodyne Research, Inc. (ARI) that is the most widely used thermal vaporization AMS. The AMS uses aerodynamic lens inlet technology together with thermal vaporization and electron-impact mass spectrometry to measure the real-time non-refractory (NR) chemical speciation and mass loading as a function of particle size of fine aerosol particles with aerodynamic diameters between similar to 50 and 1,000 nm. The original AMS utilizes a quadrupole mass spectrometer (Q) with electron impact (EI) ionization and produces ensemble average data of particle properties. Later versions employ time-of-flight (ToF) mass spectrometers and can produce full mass spectral data for single particles. This manuscript presents a detailed discussion of the strengths and limitations of the AMS measurement approach and reviews how the measurements are used to characterize particle properties. Results from selected laboratory experiments and field measurement campaigns are also presented to highlight the different applications of this instrument. Recent instrumental developments, such as the incorporation of softer ionization techniques (vacuum ultraviolet (VUV) photo-ionization, Li(+) ion, and electron attachment) and high-resolution ToF mass spectrometers, that yield more detailed information about the organic aerosol component are also described. (c) 2007 Wiley Periodicals, Inc.

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Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer

Every year, from December to April, anthropogenic haze spreads over most of the North Indian Ocean, and South and Southeast Asia. The Indian Ocean Experiment (INDOEX) documented this Indo-Asian haze at scales ranging from individual particles to its contribution to the regional climate forcing. This study integrates the multiplatform observations (satellites, aircraft, ships, surface stations, and balloons) with one- and four-dimensional models to derive the regional aerosol forcing resulting from the direct, the semidirect and the two indirect effects. The haze particles consisted of several inorganic and carbonaceous species, including absorbing black carbon clusters, fly ash, and mineral dust. The most striking result was the large loading of aerosols over most of the South Asian region and the North Indian Ocean. The January to March 1999 visible optical depths were about 0.5 over most of the continent and reached values as large as 0.2 over the equatorial Indian ocean due to long-range transport. The aerosol layer extended as high as 3 km. Black carbon contributed about 14% to the fine particle mass and 11% to the visible optical depth. The single-scattering albedo estimated by several independent methods was consistently around 0.9 both inland and over the open ocean. Anthropogenic sources contributed as much as 80% (±10%) to the aerosol loading and the optical depth. The in situ data, which clearly support the existence of the first indirect effect (increased aerosol concentration producing more cloud drops with smaller effective radii), are used to develop a composite indirect effect scheme. The Indo-Asian aerosols impact the radiative forcing through a complex set of heating (positive forcing) and cooling (negative forcing) processes. Clouds and black carbon emerge as the major players. The dominant factor, however, is the large negative forcing (-20±4 W m^(−2)) at the surface and the comparably large atmospheric heating. Regionally, the absorbing haze decreased the surface solar radiation by an amount comparable to 50% of the total ocean heat flux and nearly doubled the lower tropospheric solar heating. We demonstrate with a general circulation model how this additional heating significantly perturbs the tropical rainfall patterns and the hydrological cycle with implications to global climate.

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Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze

Plausible estimates for the effect of soot on snow and ice albedos (1.5% in the Arctic and 3% in Northern Hemisphere land areas) yield a climate forcing of +0.3 W/m2 in the Northern Hemisphere. The “efficacy” of this forcing is ∼2, i.e., for a given forcing it is twice as effective as CO2 in altering global surface air temperature. This indirect soot forcing may have contributed to global warming of the past century, including the trend toward early springs in the Northern Hemisphere, thinning Arctic sea ice, and melting land ice and permafrost. If, as we suggest, melting ice and sea level rise define the level of dangerous anthropogenic interference with the climate system, then reducing soot emissions, thus restoring snow albedos to pristine high values, would have the double benefit of reducing global warming and raising the global temperature level at which dangerous anthropogenic interference occurs. However, soot contributions to climate change do not alter the conclusion that anthropogenic greenhouse gases have been the main cause of recent global warming and will be the predominant climate forcing in the future.

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Soot climate forcing via snow and ice albedos

[1] Simultaneous measurements of atmospheric organic and elemental carbon (OC and EC) were taken during winter and summer seasons at 2003 in 14 cities in China. Daily PM2.5 samples were analyzed for OC and EC by the Interagency Monitoring of Protected Visual Environments (IMPROVE) thermal/optical reflectance protocol. Average PM2.5 OC concentrations in the 14 cities were 38.1 μg m−3 and 13.8 μg m−3 for winter and summer periods, and the corresponding EC were 9.9 μg m−3 and 3.6 μg m−3, respectively. OC and EC concentrations had summer minima and winter maxima in all the cities. Carbonaceous matter (CM), the sum of organic matter (OM = 1.6 × OC) and EC, contributed 44.2% to PM2.5 in winter and 38.8% in summer. OC was correlated with EC (R2: 0.56–0.99) in winter, but correlation coefficients were lower in summer (R2: 0.003–0.90). Using OC/EC enrichment factors, the primary OC, secondary OC and EC accounted for 47.5%, 31.7% and 20.8%, respectively, of total carbon in Chinese urban environments. More than two thirds of China's urban carbon is derived from directly emitted particles. Average OC/EC ratios ranged from 2.0 to 4.7 among 14 cities during winter and from 2.1 to 5.9 during summer. OC/EC ratios in this study were consistent with a possible cooling effect of carbonaceous aerosols over China.

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Spatial and seasonal distributions of carbonaceous aerosols over China

The effect of atmospheric aerosols and regional haze from air pollution on the yields of rice and winter wheat grown in China is assessed. The assessment is based on estimates of aerosol optical depths over China, the effect of these optical depths on the solar irradiance reaching the earth’s surface, and the response of rice and winter wheat grown in Nanjing to the change in solar irradiance. Two sets of aerosol optical depths are presented: one based on a coupled, regional climate/air quality model simulation and the other inferred from solar radiation measurements made over a 12-year period at meteorological stations in China. The model-estimated optical depths are significantly smaller than those derived from observations, perhaps because of errors in one or both sets of optical depths or because the data from the meteorological stations has been affected by local pollution. Radiative transfer calculations using the smaller, model-estimated aerosol optical depths indicate that the so-called “direct effect” of regional haze results in an ≈5–30% reduction in the solar irradiance reaching some of China’s most productive agricultural regions. Crop-response model simulations suggest an ≈1:1 relationship between a percentage increase (decrease) in total surface solar irradiance and a percentage increase (decrease) in the yields of rice and wheat. Collectively, these calculations suggest that regional haze in China is currently depressing optimal yields of ≈70% of the crops grown in China by at least 5–30%. Reducing the severity of regional haze in China through air pollution control could potentially result in a significant increase in crop yields and help the nation meet its growing food demands in the coming decades.

https://www.pnas.org/content/pnas/96/24/13626.full.pdf

Case study of the effects of atmospheric aerosols and regional haze on agriculture: an opportunity to enhance crop yields in China through emission controls?

X. Zhou

Papers

Case study of the effects of atmospheric aerosols and regional haze on agriculture: an opportunity to enhance crop yields in China through emission controls?